ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Hongmei Dai,Yue Xu,Yongchao Han,Shixiong Sun,Xiaolin Zhang,Fangyu Xiong,Chao Huang,Chun Fang,Jiantao Han,Paul K. Chu
Superior specific capacity, high-rate capability, and long-term cycling stability are essential to anode materials in sodium-ion batteries, and conductive metal–organic frameworks (cMOF) with good electronic and ionic conductivity may satisfy these requirements. Herein, conductive neodymium cMOF (Nd-cMOF) produced in situ on the zeolitic imidazolate framework (ZIF)-derived carbon fiber (ZIF-CFs) platform is used to synthesize the Nd-cMOF/ZIF-CFs hierarchical structure. Four types of ZIFs with different pore diameters are prepared by electrospinning. In this novel structure, ZIF-CFs provide the electroconductivity, flexible porous structure, and mechanical stability, while Nd-cMOF provides the interfacial kinetic activity, electroconductivity, ample space, and volume buffer, consequently giving rise to robust structural integrity and excellent conductivity. The sodium-ion battery composed of the Nd-cMOF/ZIF-10-CFs anode has outstanding stability and electrochemical properties, such as a specific capacity of 480.5 mAh g–1 at 0.05 A g–1 as well as capacity retention of 84% after 500 cycles.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xionghui Ma,Jinsheng Kang,Yuwei Wu,Chaohai Pang,Shuhuai Li,Jianping Li,Yuhao Xiong,Jinhui Luo,Mingyue Wang,Zhi Xu
The analytical functionalization of metal organic frameworks (MOFs) has been an extremely attractive topic in photoelectrochemical (PEC) sensing. However, most PEC sensors based on photoactive MOFs are more focused on the acquisition and amplification of semiconductor photoelectric signals, and the study of affinity mechanisms for specific targets is more limited. Here, we find that PCN-224 (Zn) can effectively sense organophosphorus structures through a multicenter affinity mechanism, as evidenced by x-ray photoelectron spectroscopy (XPS) and computational chemistry. Further, we coupled PCN-224(Zn) to Nb 4 C 3 to form a Schottky junction that enhances the photoelectric signal response of the sensor. In particular, the heterojunction exhibited a higher photocurrent density than pristine PCN-224(Zn) (17.3 μA vs. 26.5 μA cm −2 ). On the basis, we developed a novel MOF-based polycentric-affinity PEC sensing strategy for dimethoate (DIM) detection in concert with molecular imprinting technology. The affinity effects of the Lewis acidic center sites (Zn(II), Zr(IV)) and spatial matching through molecular imprinting synergistically ensure that DIM is precisely captured. Ultimately, a trace DIM-PEC sensor was constructed by a competitive strategy using dopamine as an electron donor. The photocurrent intensity was linearly related to the logarithm of DIM concentration in the range of 0.1 nM to 1000 nM, with a low detection limit of 26.1 pM (3σ/S). This study demonstrates the potential of bifunctional polycentric-affinity MOF in the PEC sensing.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Qun Liu,Kun Xu,Guangxu Hu,Fanming Zeng,Xiao Li,Chun Li,Yu Zhang
MIL-101(Cr)/polyacrylamide/chitosan (named as MIL-101(Cr)/PAM/CSA) composite aerogel with large surface area is synthesized by incorporating MIL-101(Cr) into polyacrylamide/chitosan composite aerogel and used for efficient 2, 4-Dichlorophenoxyacetic acid adsorption. MIL-101(Cr)/PAM/CSA and polyacrylamide/chitosan composite aerogels exhibit good underwater superelastic properties with multi-level network synergistic cross-linking. After introducing MIL-101(Cr) with the mass loading of 30%, the specific surface area of the composite aerogels enlarge from 58.15 m 2 g −1 to 310.94 m 2 g −1 . MIL-101(Cr)/PAM/CSA exhibits high adsorption capacity of 302.45 mg g −1 for 2, 4-Dichlorophenoxyacetic acid (2, 4-D) and stable recycling capability. This work provides a general and effective method to synthesize composite aerogel with underwater superelastic properties, hierarchical pores and large surface area, promising to realize regeneration after compression with reduced solvent usage and costs.
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Nanoscale
·
2021
·Vol. 14
·期 5
·1796-1806
·
IF 7.79
Wenyan Yin,Milin Zhang,Jingyuan Liu,Khaled Tawfik Alali,Jing Yu,Jiahui Zhu,Peili Liu,Rumin Li,Jun Wang
Electrochemical sensors using ionic liquids as electrolytes for oxygen detection are now getting more and more attention. Recently, an ionic liquid combined with an electrochemically active catalyst system has become popular for boosting the sensing performance of oxygen sensors. In this work, the imidazolyl-based ionic liquid 1-butyl-2,3-dimethylimidazole bis((trifluoromethyl)sulfonyl)imide [Bmmim][TFSI] is first prepared by a facile two-step method. Subsequently, a transition metal and N-codoped porous carbon oxygen reduction electrochemical catalyst Cu–N/C is synthesized by calcining the Cu-doped ZIF-8 precursor and then blending it in different ratios with the ionic liquid [Bmmim][TFSI] as composite electrolytes for oxygen detection. The composite electrolyte Cu–N/C/[Bmmim][TFSI] exhibits increased responses in cyclic voltammetry (CV) and chronoamperometry (CA) relative to that of the pure ionic liquid. Furthermore, the CV and CA data show that 6% Cu–N/C/[Bmmim][TFSI] has the optimum oxygen sensing response with an enhanced reduction peak current, a sensitivity of 0.1678 μA/[% O2] and a good linear fitting coefficient of 0.9991. In conclusion, the results confirm the success of using Cu–N/C as an electrochemical catalyst composed of the Cu–N/C/[Bmmim][TFSI] electrolyte for improving the responsivity, stability and sensitivity towards a wide range of oxygen concentrations.
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Reaction Chemistry & Engineering
·
2021
·Vol. 7
·期 2
·275-283
·
IF 4.239
Yan Zhang,Bi-Cong Wang,Po Wang,Xiao-Jie Ju,Mao-Jie Zhang,Rui Xie,Zhuang Liu,Wei Wang,Liang-Yin Chu
Uniform hydrogel microparticles with MOF nanoparticles for molecular co-confinement of cascade enzymes are developed by droplet microfluidics to achieve enhanced stability and reusability under harsh conditions. Water-swollen polyacrylamide hydrogel is used for constructing the microparticles; while microporous zeolitic imidazolate framework-8 (ZIF-8) nanoparticles are incorporated in the hydrogel networks for multi-enzyme co-confinement. With the ZIF-8 nanoparticles as armour, the multiple enzymes in the microparticles show good stability for efficient biocatalytic cascades under harsh conditions. This is demonstrated by using glucose oxidase (GOx) and horseradish peroxidase (HRP) as typical cascade enzymes. The hydrogel microparticles with both GOx and HRP confined in their ZIF-8 nanoparticles exhibit enhanced stability for efficient biocatalytic cascades and storage, after treatment under harsh conditions involving high temperature, UV light, and protease. Moreover, the hydrogel microparticles allow easy recycling and good reusability after repeated treatment at high temperature (80 °C). This work provides a simple and efficient strategy to create multiple-enzyme-loaded microcarriers with good stability and reusability for biocatalytic cascades.
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Molecular Catalysis
·
2023
·
IF 4.6
Liqiang Ma,Pengpeng Wei,Jingfang Li,Xue Lu,Guangming Li
Aerobic oxidative desulfurization (AODS) is a promising deep desulfurization technique that can efficiently remove organosulfur compounds under mild conditions. In this study, a one-pot hydrothermal method was designed to encapsulate a quaternary heteropolyacid H 4 PVMo 4 W 7 O 40 (PVMo 4 W 7 ) into rht -MOF-1 { rht -MOF-1 = [Cu 6 O(TZI) 3 (H 2 O) 6 ] 4 ⋅nH 2 O}, and the single crystal structure of H 4 PVMo 4 W 7 O 40 @ rht -MOF-1 ( 1 ) indicated that PVMo 4 W 7 was effectively encapsulated within cage C of rht -MOF-1. Further, a similar one-pot hydrothermal reaction was employed to introduce acetic acid, resulting in the synthesis of defective H 4 PVMo 4 W 7 O 40 @ rht -MOF-1-De ( 1 - De ). 1 - De was characterized using various techniques such as FT-IR, XRD, TGA, XPS, and EPR. In comparison with 1, 1 - De exhibited numerous defect sites, high porosity, high surface area, high Mo 5+ ion content, well-dispersed PVMo 4 W 7 , and abundant oxygen vacancies, leading to efficient AODS capability. When applied as catalyst, 1 - De demonstrated high catalytic activity and good recyclability for the oxidation of dibenzothiophene (DBT) and 4,6-dimethyl dibenzothiophene (4,6-DMDBT) under air atmosphere. Strikingly, the removal rates of DBT and 4,6-DMDBT reached 99 % and 96 %, respectively under optimized conditions.
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LUMINESCENCE
·
2023
·Vol. 39
·期 2
·e4651
·
IF 2.9
Weiwei Yuan,Shuhuai Li,Xionghui Ma,Chaohai Pang,Yuwei Wu,Mingyue Wang,Bei Li
The luminescence performance of fluorescent reagents plays a crucial role in fluorescence analysis. Therefore, in this study, a novel bi-ligand Zn-based metal–organic framework, Au nanoparticle (NP) fluorescent material was synthesized using a hydrothermal method with Zn as the metal source. Simultaneously, a DNA aptamer was introduced as a molecular recognition element to develop a Zn-based MOF@Au NPs/DNA aptamer fluorescent probe for the ultra-trace detection of thiamethoxam residues in agricultural products. The probe captured different concentrations of the target molecule, thiamethoxam, through the DNA aptamer, causing a conformational change in the DNA aptamer and bursting the fluorescence of the probe, therefore establishing a fluorometric method for thiamethoxam detection. This method is highly sensitive due to the excellent luminescence properties of the Zn-based MOF@Au NPs, and the DNA aptamer can specifically recognize thiamethoxam, offering high selectivity. The linear range of the method was 2.5–6000 × 10 −11 mol L −1 , with a detection limit of 8.33 × 10 −12 mol L −1 . This method was applied to the determination of actual samples, such as bananas, and the spiked recovery rate was found to be in the range 84.05–109.07%. Overall, the proposed probe has high sensitivity, high selectivity, and easy operation for the detection of thiamethoxam residues in actual samples.
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DALTON TRANSACTIONS
·
2023
·Vol. 53
·期 4
·1757-1765
·
IF 4
Zheng Zhang,Lei Han,Kai Tao
Exploring non-noble metal dual-functional electrocatalysts with high activity and stability for water splitting is highly desirable. In this study, using zeolitic imidazolate framework-L (ZIF-L) nanoarrays as the precursor, manganese oxide-decorated porous nickel–cobalt phosphide nanosheet arrays have been prepared on nickel foam (denoted as MnOx/NiCoP/NF) through cation etching, phosphorization and electrodeposition, which are utilized as an efficient dual-functional electrocatalyst for overall water splitting. The hierarchical porous nanosheet arrays provide abundant active sites for the electrochemical process, while the MnOx modification induces strong interfacial interaction, benefiting charge transfer. Thus, the MnOx/NiCoP/NF exhibits excellent electrocatalytic activity toward the hydrogen evolution reaction (HER, overpotential of 93 mV at 10 mA cm−2), oxygen evolution reaction (OER, overpotential of 240 mV at 10 mA cm−2) and overall water splitting (cell voltage of 1.59 V at 10 mA cm−2). Furthermore, it shows superior stability during continuous overall water splitting for 200 h. This work provides a simple and effective approach for developing efficient non-noble metal dual-functional catalysts for overall water splitting.
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ACS Nano
·
2026
·
IF 17.3
Li Zhongbing,Huang Lei,Xu Chenchen,Zhang Wenyan,Xu Lizhi,Chu Yuting,Ke Zhuo,Zhang Zhen,Liu Deguang,Li Chuang,Fu Yao
The performance of high-rate batteries is primarily constrained
by inefficient ion transport across the separator/electrolyte interface.
Commercial polyolefin separators depend on passive microporous diffusion
and are unable to actively guide Li + migration pathways,
leading to concentration polarization, dendritic growth, and fast
capacity decay. Herein, we present a hierarchical cooperative transport
strategy that enables active guidance and directed migration of Li + through the construction of a multihub, cross-scale “ionic
highway”. In this strategy, metal–organic frameworks
(MOFs) and carboxylated cellulose nanocrystals (C–CNC) are
integrated to exert a synergistic effect, leading to the design and
fabrication of a poly(vinyl alcohol) (PVA)-based electrospun composite
separator (PCUS). Nanoscale MOFs serve as the primary pathways for
selective PF 6 – adsorption and facilitate
Li + solvation-shell regulation, thereby accelerating overall
ion migration kinetics. Concurrently, abundant carboxyl groups on
C–CNC serve as auxiliary hopping sites, lowering ion transport
activation energy. Combined with the separator’s inherent microporosity,
these components establish hierarchical conduction paths from the
nano- to microscale, significantly enhancing overall transport efficiency.
The separator demonstrates a high ionic conductivity of 2.664 mS cm –1 and a Li + transference number of 0.81.
Assembled into Li|PCUS|LiFePO 4 cells, it delivers 120.3
mAh g –1 at 5C, retaining 98.1% capacity over 300
cycles. NCM811|PCUS|Graphite full cell achieves a capacity retention
of 95.9% at 1C/150 cycles. In addition, PCUS shows excellent dendrite
suppression, enabling stable lithium deposition for over 2000 h at
0.2 mA cm –2 . This work offers a rational design
paradigm to address ion transport limitations and a sustainable route
toward high-safety, long-lifespan energy storage.
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Progress in Natural Science-Materials International
·
2023
·
IF 4.7
Lin Zhang,Jun Chen,Lai-Bo Song,Jun-Jie Pan,Qing Luo
Developing effective and stable photocatalysts for organic pollutants degradation are still a big challenge in practical water treatment now. In this work, La doped ZnO–TiO 2 composite (La/ZnO–TiO 2 ) were successfully fabricated by using PVP modified ZIF-8/TiO 2 as template via the absorption and pyrolysis routes. All as-fabricated materials were analyzed by XRD , SEM, TEM , BET, XPS , UV–vis absorption spectra and ESR spectra. PVP modified ZIF-8/TiO 2 was fully transferred into ZnO–TiO 2 after being pyrolyzed at high temperature under air atmosphere. The doping of La can make ZnO–TiO 2 exhibiting red-shifted, which is attributed to the capture of photo-generated electrons by La, leading to the effective separation between photo-generated electrons and holes. Furthermore, the photocatalytic performance of all as-fabricated materials were explored by degradation of tetracycline (TC) solution under UV light irradiation. La/ZnO–TiO 2 exhibits excellent stability. And the photocatalytic degradation rate of La/ZnO–TiO 2 is 99.2%, which is even higher than ZnO (87.4%), ZnO–TiO 2 (87.4%), P25 (TiO 2 ) (92.7%). More than that, the effect of catalyst's dose, effect of TC concentration and effect of pH for TC degradation have been well explored. The excellent photocatalytic performance of La/ZnO–TiO 2 makes it possible to be applied for degradation of organic pollutants in practice.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiabing Luo,Xingzhao Wang,Shutao Wang,Wenle Li,Yanpeng Li,Tingyong Wang,Fengqi Xu,Yang Liu,Yan Zhou,Jun Zhang
Inducing the surface reconstruction of spinels is critical for improving the electrocatalytic oxygen evolution reaction (OER) activity. Herein, S-doped NiCo 2 O 4 hollow cubic nanocage was synthesized by anion etching Metal-Organic Frameworks (MOFs) template and air annealing strategies. The hollow structure possesses a large specific surface area and pore size, facilitating active site exposure and mass transport. S 2− doping regulates the electronic structure, reducing the oxidation potential of Ni sites during the OER process, thus promoting the surface reconstruction into γ-NiOOH active species. Meanwhile, S 2− doping enhances conductivity, accelerating interfacial charge transfer. As a result, S-NiCo 2 O 4 -6 exhibits superior OER activity (262 mV overpotential @ 10 mA cm −2 ) and stability in 1.0 M KOH solution. Furthermore, 20 % Pt/C‖S-NiCo 2 O 4 -6 only needs 1.832 V to achieve 50 mA (the electrochemical active area is 4 cm 2 ) in a homemade anion exchange membrane (AEM) electrolyzer. This work proposes a novel approach for preparing efficient anion-doped spinel-based OER electrocatalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Yi Zhao,Shuang Wang,Zhiheng Zhang,Yidong Hu,Kai Ge,Binyuan Liu,Yongfang Yang
Metal-organic framework (MOF) layers were grown in situ from 2D transition metal carbides (MXenes, Ti 3 C 2 T x ) at room temperature to obtain the two-dimensional (2D) Ti 3 C 2 T x @MOF heterostructures with a tightly connected interface. This interface provided more titanium atoms in the low-valence state in comparison to the original Ti 3 C 2 T x , thus facilitating more electron transfer from Ti 3 C 2 T x to MOF-(Fe/Co) nanosheets . The charge density difference and density functional theory results disclosed that Ti 3 C 2 T x could modulate the electronic density around the active sites and lower ΔG H * energy barrier of 2D MOF-(Fe/Co) nanosheets towards the improved hydrogen evolution reaction (HER) activity. The obtained 2D Ti 3 C 2 T x @MOF heterostructures exhibited a much higher HER activity in 1 M KOH electrolyte (with the overpotential of 104 mV at 10 mA/cm 2 and Tafel slope of 79 mV/dec) than those of 2D Ti 3 C 2 T x @MOF-TH, 2D MOF nanosheets , and Ti 3 C 2 T x nanosheets. This research provides a basis for developing superior 2D MOFs, which can enhance HER properties through efficient electronic transport at the heterojunction interface.
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